Photoinduced Anomalous Coulomb Blockade and the Role of Triplet States in Electron Transport through an Irradiated Molecular Transistor

Bo Fu, Martín A. Mosquera, George C. Schatz, Mark A. Ratner, Liang Yan Hsu*

*Corresponding author for this work

Research output: Contribution to journalArticle

4 Scopus citations

Abstract

In this study, we explore photoinduced electron transport through a molecule weakly coupled to two electrodes by combining first-principles quantum chemistry calculations with a Pauli master equation approach that accounts for many-electron states. In the incoherent limit, we demonstrate that energy-level alignment of triplet and charged states plays a crucial role, even when the rate of intersystem crossing is much smaller than the rate of fluorescence. Furthermore, the field intensity dependence and an upper bound to the photoinduced electric current can be analytically derived in our model. Under an optical field, the conductance spectra (charge stability diagrams) exhibit unusual Coulomb diamonds, which are associated with molecular excited states, and their widths can be expressed in terms of energies of the molecular electronic states. This study offers new directions for exploring optoelectronic response in nanoelectronics.

Original languageEnglish (US)
Pages (from-to)5015-5023
Number of pages9
JournalNano letters
Volume18
Issue number8
DOIs
StatePublished - Aug 8 2018

Keywords

  • Jablonksi diagram
  • Molecular electronics
  • energy conversion
  • optoelectronics
  • quantum transport

ASJC Scopus subject areas

  • Bioengineering
  • Chemistry(all)
  • Materials Science(all)
  • Condensed Matter Physics
  • Mechanical Engineering

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